As electrical multi-terminal devices are made smaller, the contacts to the electrodes are critical to their overall performance and are typically ‘weak links’ where significant wasteful deleterious dissipation occurs (Emerging Research Materials International Technology Roadmap for Semiconductors 2011). This obstacle to device-size reduction is a major impediment to the utilization and control of high-mobility materials such as carbon nanotubes (CNTs) and graphene as device channels for high-frequency applications and in reducing their deleterious excess heat production (Franklin et al. Nature Nanotechnology 2010, 5, 858-862; Xia et al. Nature Nanotechnology 2011, 6, 179-184). Maintaining the same crystallographic orientation at all electrode interfaces of a device could allow for the emergence of quantum behavior, such as ballistic and phase coherent transport. Such quantum transport could achieve new functionality, such as resonant tunneling and negative differential resistance, that could be useful for high-speed applications. Thus, a method to tune and significantly increase electrical coupling between high-mobility electrodes and channels is crucial for reducing the contact resistances and widening the possible functions of nanoscale devices.